No. Fermi particles have half-integral spin. These are the particles that obey the Pauli exclusion principle. The spin can be 1/2, 3/2, etc. You can have nuclei, atoms, or individual subatomic particles ( like electrons, neutrons and protons - all are spin 1/2). Nuclei with an odd number of nucleons (spin-1/2) will have half-integral spin. But depending on the structure, you can get larger values - Cs-133, for example, has nuclear spin 7/2.
You also have Bosons, which have integral spin. 0, 1, 2... Mesons are spin 0. Nuclei with an even number of nucleons will have integral spin.
Rb-87 has 87 nucleons, and the nucleus has spin 3/2. But the atom itself, because it has 37 electrons (i.e. an odd number), has an integral spin.
You can't choose the spin of the atom. You can only choose the orientation (i.e. the direction the angular momentum vector points)